Molecular Dynamics in a Grand Ensemble: Bergmann-Lebowitz model and Adaptive Resolution Simulation

TL;DR

This paper explores the Bergmann-Lebowitz model for open system molecular dynamics, demonstrating its utility in defining physical quantities and calculating equilibrium correlations within the GC-AdResS framework, with numerical results for water.

Contribution

It introduces the application of the Bergmann-Lebowitz model to open system simulations, linking it with the GC-AdResS method for improved physical quantity definitions.

Findings

The Bergmann-Lebowitz model can be used to define physical quantities in open systems.

Application of the model within GC-AdResS enables calculation of equilibrium time correlation functions.

Numerical results for liquid water validate the approach.

Abstract

This article deals with the molecular dynamics simulation of open systems that can exchange energy and matter with a reservoir; the physics of the reservoir and its interactions with the system are described by the model introduced by Bergmann and Lebowitz.Despite its conceptual appeal, the model did not gain popularity in the field of molecular simulation and, as a consequence, did not play a role in the development of open system molecular simulation techniques, even though it can provide the conceptual legitimation of simulation techniques that mimic open systems. We shall demonstrate that the model can serve as a tool to devise both numerical procedures and conceptual definitions of physical quantities that cannot be defined in a straightforward way by systems with a fixed number of molecules. In particular, we discuss the utility of the Bergmann-Lebowitz (BL) model for the calculation of equilibrium time correlation functions within the Grand Canonical Adaptive Resolution method (GC-AdResS) and report numerical results for the case of liquid water.